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The integration of graphene with diamond holds great promise for all-carbon materials, yet the precise mechanism governing graphene formation on diamond has remained unclear due to the lack of direct experimental evidence. Conventional preparation methods often rely on empirical annealing parameters. In this study, the catalytic transformation from diamond into graphene or graphite (nickel (Ni) as a catalyst) is investigated through in-situ heating transmission electron microscopy (TEM). We demonstrate that the transition proceeds via a metal-induced solid-state mechanism that is driven by Ni catalysis and reaction-diffusion between Ni and carbon (C) atoms at elevated temperatures. Key processes include Ni grain migration and C–Ni interdiffusion. The annealing duration significantly influences the location and number of graphene layers. Notably, prolonged annealing causes the development of graphene on the Ni surface, whereas rapid, short-term annealing results in the formation of graphene at the diamond/Ni interface. Extended high-temperature exposure increases the number of graphene layers, potentially facilitating graphite formation. Ab initio simulations reveal the polymerization pathway of carbon within the Ni(C) solid solution during graphene nucleation. These insights provide valuable guidance for designing application-specific graphene-on-diamond (GOD) structures, promoting the development of advanced carbon-based technologies.

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• In Copyright
  

Keyword: diamond

Date published: 2025-12-27

Publisher: Elsevier BV

Journal:

• Progress in Solid State Chemistry (ISSN: 00796786) vol. 82 100562

Funding:

• HORIZON EUROPE Framework Programme 101027489
• HORIZON EUROPE Framework Programme 101131231
• Horizon 2020 Framework Programme
• Beijing University of Technology
• National Key Research and Development Program of China Stem Cell and Translational Research 2016YFE0133200
• HORIZON EUROPE Framework Programme 734578
• National Key Research and Development Program of China

Manuscript type: Author's version (Submitted manuscript)

MDR DOI: https://doi.org/10.48505/nims.6407

First published URL: https://doi.org/10.1016/j.progsolidstchem.2025.100562

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Updated at: 2026-07-14 11:04:26 +0900

Published on MDR: 2026-07-14 12:30:09 +0900